RESEARCH ARTICLE

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Highly Sodiophilic Heterostructures Toward Dendrite-Free

Sodium Metal Batteries
Yongshi Yu, Shitan Xu, Yang Yang, Yu Yao, Ghulam Ali, Zetian Tao, Xianhong Rui,*
and Yan Yu*

1. Introduction
The utilization of Al current collector for the sodium
The large-scale development of lithium-
deposition is considered ideal for achieving a low-cost, high-energy-density
ion batteries is currently constrained by
sodium metal battery. However, the poor affinity between sodium and Al the shortage and uneven distribution
leads to uneven sodium plating/stripping, which poses a significant challenge of lithium resources.[1–5] Researchers
in the pursuit of a stable sodium metal anode. Herein, a heterostructure have turned their attention to sodium
(V/VOx )-modified Al current collector is proposed, which effectively enables (Na), which shares similar physical and
a highly reversible Na plating/stripping process, and inhibits Na dendrites chemical properties with lithium and is
more abundant, wide distributed, and
growth. Experimental results and theoretical calculations demonstrate
cost-effective.[6–10] Therefore sodium-
that the V/VOx @Al not only exhibits strong sodiophilicity, but also ensures ion batteries (SIBs) are regarded as one
a uniform current density distribution. Thanks to these merits, the assembled of the highly promising energy storage
cells demonstrate excellent performances with low nucleation overpotential candidates for the next generation. In
(11 mV at 1 mA cm−2 ), and long cycle life (2750 h) with minimal voltage recent years, SIBs have made remarkable
progress with the continuous progress
polarization (13 mV at 1 mA cm−2 ). More impressively, the assembled full cell
of science and technology. However, the
displays remarkable stability, sustaining 1400 cycles at 10 C. This work provides energy density of SIBs is low,[11–15] making
valuable insights for the development of more stable sodium metal batteries. it challenging to meet the requirements
for prolonged standby time in electronic
devices and long-range transportation. Na
metal is notable for its high theoretical capacity (1166 mA h g−1 )
Y. Yu, S. Xu, Y. Yang, X. Rui
Jieyang Branch of Chemistry and Chemical Engineering Guangdong and a low redox potential (−2.71 V versus SHE).[16,17] These prop-
Laboratory (Rongjiang Laboratory) erties make Na metal a highly promising anode, and its directly
Jieyang 515200, China assembly with a suitable cathode into a full cell can significantly
E-mail: xhrui@gdut.edu.cn increase the energy density of sodium-based batteries.[18] This ad-
Y. Yu, S. Xu, Y. Yang, X. Rui vantage makes sodium metal batteries (SMBs) have great poten-
Guangdong Provincial Key Laboratory on Functional Soft Condensed
Matter tial for application in energy storage.
School of Materials and Energy The practical application of SMBs, however, has faced obsta-
Guangdong University of Technology cles due to their low Columbic efficiency (CE) and short lifes-
Guangzhou 510006, China pan. These issues can be attributed to the factors of high reactiv-
Y. Yao, Y. Yu ity with the electrolyte, large volume fluctuation of sodium, and
Hefei National Research Center for Physical Sciences at the Microscale
uneven sodium deposition/exfoliation behavior.[19–29] The choice
iChEM (Collaborative Innovation Center of Chemistry for Energy Materials)
Department of Materials Science and Engineering of current collectors as plating substrates significantly affects the
CAS Key Laboratory of Materials for Energy Conversion behavior of Na plating and stripping.[30,31] In the initial nucle-
University of Science and Technology of China ation stage, Na ions tend to form nuclei at rough spots caused
Hefei, Anhui 230026, China by bumps and dents on the surfaces of conventional planar cur-
E-mail: yanyumse@ustc.edu.cn
rent collectors.[32,33] As the growth progresses, these nuclei act
G. Ali
U.S.-Pakistan Center for Advanced Studies in Energy as charge centers, attracting Na+ due to the enhancement of lo-
National University of Sciences and Technology cal electric field at these points.[34] This behavior results in an
Islamabad 44000, Pakistan uneven distribution of Na+ , and consequently, occurring Na den-
Z. Tao drites. Therefore, great efforts have been made to achieve a uni-
School of Resources form distribution of current density on the current collector. For
Environment and Safety Engineering
example, Liu et al.[32] successfully prepared porous Al by electro-
University of South China
Hengyang, Hunan 421001, China chemical corrosion. Compared with planar Al current collector, it
offers a larger surface area, which not only increases the sites for
The ORCID identification number(s) for the author(s) of this article Na nucleation, but also reduces the effective current density and
can be found under https://doi.org/10.1002/adfm.202401914
Na+ flux distribution. However, challenges with this porous Al
DOI: 10.1002/adfm.202401914

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Figure 1. a–c) SEM images of the V/VOx @Al foil at different magnifications. d) The cross-sectional SEM image, e) XRD pattern, and f) XPS V 2p
spectrum of the V/VOx @Al foil. g) HRTEM images of the V/VOx @Al foil, and h) the corresponding SAED pattern.
current collector are poor mechanical strength and hard to main-
tain the structure integrity. Similarly, in a study by Wu et al.,[35]
vertically grown ZnO nanorod arrays on copper foam (CF@ZnO)
were prepared by a simple chemical deposition method. These
ZnO nanorod arrays demonstrated the ability to reduce local cur-
rent density and homogenize the electric field distribution to
achieve uniform Na deposition. However, the application of 3D
current collectors has its drawbacks. Although 3D current collec-
tors have the advantage of providing large surface area, they re-
quire more electrolyte to wet due to their complex microstructure
and increased interface reactions. This in turn increases the risk
of electrolyte decomposition, especially in the areas of uneven
current distribution and at high temperatures. Electrolyte degra-
dation can lead to continuous capacity decay, which can impair
the service life of the battery.[36,37]
Introducing sodiophilic materials onto planar current col-
lectors is an effective approach to reduce current density. For
example, Chen et al.[38] successfully deposited Zn and SnO2
onto the surface of Cu foil by magnetron sputtering, creating
a porous structure that effectively reduces local current density.
This method enables the bottom-up deposition of Na, showcas-
ing superior electrochemical performance. However, it utilizes
relatively expensive copper foil and requires multiple sputtering
processes to construct the porous structure, making it challeng-
ing to execute. Therefore, our proposed alternative method aims
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to homogenize the current density distribution by a more cost-
effective way.
Herein, we successfully developed a V/VOx (x = 0.2-0.5) het-
erostructure onto the surface of the commercialized and inex-
pensive Al foil (V/VOx @Al) by magnetron sputtering and cal-
cination. Vanadium and vanadium oxides are found to exhibit
strong sodiophilic properties, which can effectively reduce the
Na nuclear barrier. The V/VOx heterostructure facilitates rapid
Na+ transfer and its synergistic effect of built-in electric field can
enable the uniform distribution of the current density, thereby
preventing dendritic formation during Na deposition. As a re-
sult, the V/VOx @Al presents a high average CE of 99.8% at
1 mA cm−2 /1 mAh cm−2 for 750 cycles, illustrating su-
perior Na deposition/stripping reversibility. Furthermore, the
Na@V/VOx @Al symmetric cell can be stably cycled for 2750 h
at 1 mA cm−2 /1 mA h cm−2 . Remarkably, when combined with
Na3 V2 (PO4 )3 (NVP) cathode, the Na@V/VOx @Al||NVP full cell
can operate for 1400 cycles at 10 C and maintain 97% capacity re-
tention, demonstrating excellent electrochemical performance.
2. Results and Discussion
The growth of V/VOx heterostructures on the surface of Al
foil was achieved by magnetron sputtering of vanadium on Al,
followed by an annealing process under Ar atmosphere. The
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Figure 2. a) CE and b) nucleation overpotentials of various half cells with a fixed capacity of 1 mAh cm−2 at 1 mA cm−2 . CE of various half cells at c)
2 mA cm−2 and d) 3 mA cm−2 , and the corresponding voltage-capacity profiles of V/VOx @Al cell at e) 2 mA cm−2 , and f) 3 mA cm−2 .

morphological characteristics of the Al foil and the modified Al
foil were studied by scanning electron microscopy (SEM). As
shown in Figure S1a (Supporting Information), the surface of
the Al foil is not completely flat, exhibiting areas with depres-
sions or bumps. Similarly, the surface of the V-deposited Al foil
(V@Al) is also rough (Figure S1b, Supporting Information). In
contrast, the V@Al foil after annealing displays a smoother mor-
phology, with homogeneous distribution of submicron particles
(ranging from 100 to 200 nm) on the surface (Figure 1a–c; Figure
S2a, Supporting Information). The energy-dispersive X-ray spec-
troscopy (EDS) of the V/VOx @Al foil illustrates the uniform dis-
tribution of a large number of V and O elements (Figure S2a,
Supporting Information), implying the presence of surface oxy-
gen, which is crucial for the formation of V/VOx heterostructure.
Besides, its cross-sectional SEM image (Figure 1d) and the corre-
sponding elemental mapping (Figure S2b, Supporting Informa-
tion) demonstrate that the thickness of the coating layer is ≈3 μm,
and it is in close contact with the Al foil substrate, which is con-
ducive to the improvement of structural stability and the reduc-
tion of contact resistance. Furthermore, the phase structure of
the modified Al foils was investigated by X-ray diffraction (XRD).
The XRD pattern of the magnetron sputtered Al foil (Figure S3a,
Supporting Information) exhibits peaks that corresponded to the
standard peaks of V (JCPDS No. 22–1058) as well as the standard
peaks of Al (JCPDS No. 04–0787). After annealing, as displayed
in Figure 1e, in addition to the V and Al, diffraction peaks related
to VOx phases (JCPDS No. 10–0321/75-1042/30-1425) are found.
X-ray photoelectron spectroscopy (XPS) measurement was fur-
ther conducted to reveal the composition and chemical state of
the modified foils. In the high-resolution V 2p spectrum of the
V@Al foil (Figure S3b, Supporting Information), the peaks at
512.3 and 513.3 eV correspond to the V(metal) and V2+ of V 2p3/2 ,
respectively.[39–41] For the annealed foil (Figure 1f), besides the
previous V(metal) and V2+ signals, there is a new peak detected
at 515.4 eV, corresponding to the V3+ 2p3/2 of vanadium oxides.
Furthermore, the presence of VOx and V was confirmed by high

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Figure 3. Galvanostatic cycling of symmetric cells with various electrodes a) at 1 mA cm−2 , b) 3 mA cm−2 , and c) 4 mA cm−2 (fixed capacity:1 mAh cm−2 ).
d) Rate performance of various symmetric cells at current densities ranging from 0.5 to 8 mA cm−2 .

resolution transmission electron microscope (HRTEM) and se-
lected area electron diffraction (SAED). As depicted in Figure 1g
and Figure S4 (Supporting Information), the lattice fringes mea-
suring 0.160 and 0.224 nm correspond to the (−114) and (203)
crystalline phases of VOx , respectively; on the other hand, the lat-
tice fringes of 0.214 and 0.215 nm are attributed to the (110) crys-
talline phase of V. The SAED pattern in Figure 1h also confirms
the presence of V and VOx , specifically displaying crystal faces of
V (110), as well as VOx (−115), (−114) and (203).
To explore the important role of the V/VOx layer on the reg-
ulation of reversible Na deposition, CE of Na plating/stripping
on/off bare Al, V@Al, and V/VOx @Al foils was investigated us-
ing an electrolyte of 1 m NaPF6 in diglyme, as shown in Figure 2.
The V/VOx @Al half-cell achieves high average CE of 99.8%, as
well as high stability for more than 750 cycles under 1 mA cm−2
and 1 mAh cm−2 (Figure 2a). In contrast, the bare Al and
V@Al half-cells suffer from instable CE. Figure 2b illustrates
the voltage-capacity curves of sodium deposition on various sub-
strates at 1 mA cm−2 /1 mAh cm−2 . All curves show a drop in
voltage when Na deposition begins, followed by a stable voltage
plateau, and the difference between the bottom of this voltage
drop and the voltage plateau is referred to as the nucleation over-
potential. It is found that the Na nucleation overpotential for Na
on V/VOx @Al is only 11 mV, which is much lower than that of
V@Al (35 mV) and Al (61 mV), indicating a fast nucleation ki-
netics for V/VOx @Al. Further increase of the current density to
2 and 3 mA cm−2 (Figure 2c,d), Na can be still stably cycled on
V/VOx @Al foil for 750 and 200 cycles with high average CEs of
99.9% and 99.7%, respectively. However, the CEs of bare Al and
V@Al foils fluctuate greatly due to the generation of Na den-
drites and dead sodium. Figure 2e,f and Figure S5 (Supporting
Information) show the galvanostatic voltage profiles of various
current collectors for Na plating/stripping. The voltage-capacity
curves of V/VOx @Al foil almost overlap at different cycles, while

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the bare Al and V@Al foils display large polarization and low
capacity. These results indicate that the V/VOx @Al foil has a su-
perior Na plating/stripping reversibility compared to the V@Al
and Al foils. Additionally, the V/VOx @Al synthesized in this work
has excellent plating/stripping reversibility when compared with
some reported literatures (Table S1, Supporting Information).
To further evaluate the electrochemical performance of the
three current collectors, 3 mAh cm−2 of Na was initially deposited
on them and then utilized to assemble symmetric cells. The
voltage-time profiles of various symmetrical cells at 1 mA cm−2
and 1 mAh cm−2 are shown in Figure 3a. The Na@V/VOx @Al
symmetric cell presents a small polarized voltage (13 mV) and
extremely long lifespan of 2750 h. In contrast, the Na@Al and
Na@V@Al symmetric cells exhibit larger polarized voltages and
shorter cycling lifespan of 1000 and 1600 h, respectively, demon-
strating unstable Na plating/stripping. When the current density
is increased to 3 and 4 mA cm−2 , the Na@V/VOx @Al symmet-
ric cell can still cycle steadily for 1200 and 700 h, respectively,
which are extremely longer than those of Na@Al and Na@V@Al
cells (Figure 3b,c). Furthermore, the rate capability of three sym-
metric cells with a fixed capacity of 1 mAh cm−2 at different cur-
rent densities (0.5, 1, 2, 3, 5, and 8 mA cm−2 ) was conducted
(Figure 3d). Apparently, at high rates, the Na@V/VOx @Al sym-
metric cell demonstrates significantly lower voltage hysteresis
compared to Na@V@Al and Na@Al symmetric cells. Addition-
ally, the Na@V/VOx @Al symmetric cell still maintains smooth
voltage platforms even when the current density reduces from
8 to 0.5 mA cm−2 , illustrating superior rate performance. More-
over, the Na@V/VOx @Al electrode synthesized in this work has
excellent electrochemical cycle stability compared with some lit-
eratures reported before (Table S2, Supporting Information).
The Na deposition behavior of the V/VOx heterostructure on
the electrode surface was analyzed via in situ optical measure-
ment (Figure 4a–c). And the discharge curve obtained by in situ
optical test is shown in Figure S6 (Supporting Information). Dur-
ing the entire Na deposition process, the V/VOx @Al foil consis-
tently maintains a smooth and stable surface, without any no-
ticeable formation of Na dendrites. By contrast, Na dendrites
start to appear on the surfaces of both Al and V@Al foils after
only 10 min of plating. As the deposition continues, their sur-
faces become increasingly covered with numerous dendrites by
the time 60 min have passed. Moreover, the surface morphology
of various current collectors after plating/stripping for 100 cy-
cles at 3 mA cm−2 /3 mAh cm−2 was characterized (Figure 4d–f;
Figure S7, Supporting Information). On the surfaces of Al and
V@Al foils, numerous Na dendrites can be observed. However,
the V/VOx @Al foil displays a relatively smooth and dense sur-
face without obvious Na dendrites. This may be attributed to the
fact that the V/VOx heterostructure not only reduces the Na nu-
cleation overpotential to enable Na to nucleate uniformly on its
surface, but also homogenizes the current density distribution so
that the deposition rates of Na on the surface of the heterostruc-
ture are similar, avoiding localized over-rapid deposition leading
to the formation of Na dendrites. These results demonstrate the
high effectiveness of V/VOx heterostructure in suppressing Na
dendrite growth.
The structure stability plays a crucial role in influenc-
ing the growth of Na dendrites. XRD patterns of Al, V@Al,
and V/VOx @Al foils after Na plating/stripping are shown in
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Figure 4. In situ optical detection of Na deposition on the surface of a) Al,
b) V@Al, and c) V/VOx @Al at 1 mA cm−2 . The SEM images of Na plating
on the surface of d) Al, e) V@Al, and f) V/VOx @Al at 3 mA cm−2 .
Figures 5a,b and S8 (Supporting Information). The presence of
Na, V, and VOx phases in Na@V/VOx @Al foil is found. And the
XPS spectra of V 2p and F 1s for Na@V/VOx @Al electrode after
10 cycles are exhibited in Figure 5c,d. In the high-resolution V 2p
spectrum, three peaks at 512.5, 513.4, and 515.4 eV correspond
to V(metal) , V2+ , and V3+ 2p3/2 , respectively. This result is consis-
tent with the V valence states observed in V/VOx @Al foil before
cycling, which indicates that the V/VOx heterostructure has
good structural stability. Besides, Na-F bond is detected in the
spectrum of F 1s. Furthermore, the uniform Na, F distribution in
EDS-mapping (Figure S9, Supporting Information) and the pres-
ence of Na-F band detected from Raman spectrum (Figure S10,
Supporting Information) further confirms the exitance of
NaF.[42–44] These results suggest that a NaF-rich solid electrolyte
interphase layer forms on the surface of the heterostructure after
cycling.
Electrochemical impedance spectroscopy (EIS) measurement
was performed at various temperatures to analyze Na+ transfer
kinetics at the interface between the electrolyte and substrate.
The EIS of Al, V@Al, and V/VOx @Al half cells after 5 cycles at
1 mA cm−2 /1 mAh cm−2 is presented in Figure S11 (Supporting
Information). The semicircle corresponds to the charge transfer
resistance (Rct ).[45] It is evident that the V/VOx @Al foil present
much lower Rct compared to the Al and V@Al foils. According
to the Arrhenius equation[46] and the slope of the fitted line in
Figure 5e, the calculated activation energies (Ea ) for Na+ diffusion
from the electrolyte to the substrates of Al, V@Al, and V/VOx @Al
foils are 45.47, 40.54, and 34.45 kJ mol−1 , respectively. It indi-
cates that the V/VOx heterostructure has a lower interface energy
barrier, which is conducive to reduce the initial Na nucleation
size and effectively inhibiting Na dendrite formation. Besides,
the exchange current density (Jo ) for different symmetrical cells
was determined using Tafel plots to evaluate the transportation
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Figure 5. a) The XRD pattern of the Na@V/VOx @Al electrode after 10 cycles at 3 mA cm−2 and b) the corresponding locally enlarged pattern in the 2
Theta range of 28o –44o . The XPS spectra of c) V 2p and d) F 1s for the Na@V/VOx @Al electrode after 10 cycles. e) The calculated Ea for Na+ diffusion
from electrolyte to different current collectors. f) The Tafel curves of various symmetric cells.

kinetics of Na+ . As exhibited in Figure 5f, the Na@V/VOx @Al
electrode displays a higher Jo of 2.69 mA cm−2 than that of Al
(1.00 mA cm−2 ) and V@Al (1.85 mA cm−2 ) electrodes, further
confirming its enhanced Na+ transport kinetics. Additionally, the
wettability between the electrolyte and different current collec-
tors was evaluated by measuring the contact angle in a glove box
(Figure S12, Supporting Information). The V/VOx @Al foil dis-
plays a smaller contact angle of 18° than that of V@Al foil (37°)
and Al foil (40°), suggesting that the electrolyte effectively wets
the surface of the V/VOx heterostructure.
To gain further insight into the plating behavior of Na on
the three different current collectors, the Na adsorption energies
for Al, V@Al, and V/VOx @Al foils were calculated by density
functional theory (DFT). Figures 6a–c and S13 (Supporting In-
formation) present the possible adsorption sites and the corre-
sponding adsorption energies (Eads ) of Na on the crystal planes
of Al (111), V (110), and V (110)/VOx (101) (x = 0.5). Obviously,
the Eads of Na at the most stable adsorption sites on V/VOx het-
erostructure (−3.24 eV) is larger than that on Al (−1.72 eV) and
V (−2.77 eV), indicating that Na is preferentially deposited on
V/VOx heterostructure, which is beneficial to reduce the Na nu-
cleation barrier.[45,47–50] Figure 6d shows the differential charge
density and Bader charge transfer of Na+ on various current col-
lectors. The charge transfer of Na+ on V/VOx heterostructure
(0.87 |e|) is stronger than that on Al (0.71 |e|) and V (0.75 |e|). It
indicates that the stronger sodiophilic behavior of the V/VOx @Al
foil is due to the larger charge transfer between Na+ and het-
erostructure, leading to the lower Na nucleation overpotential.[38]

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Figure 6. Adsorption sites and corresponding adsorption energies of Na on the crystal planes of a) Al (111), b) V (110), and c) V (110)/VOx (101) (x =
0.5). d) Differential charge density and Bader charge transfer of Na on various current collectors. Simulation results showing the distribution of current
density on e) Al and f) V/VOx heterostructure during Na+ deposition.

The unique advantage of the V/VOx heterostructure for the re-
versible sodium deposition was further investigated by finite el-
ement analysis (FEA), describing the variation of current den-
sity. As shown in Figure 6e,f, the color shift denotes variations in
current density, and the streamline represents the current den-
sity vector. It can be observed that the current density is no-
tably concentrated at the bulges on the Al foil (Figure 6e), where
Na+ tends to be deposited due to high current density,[51] result-
ing in uneven Na deposition and hastening the growth of Na
dendrites. In contrast, the current density distribution on the
V/VOx heterostructure is uniform (Figure 6f), indicating that the
V/VOx heterostructure can homogenize current density distribu-
tion, thereby inducing uniform Na deposition.
Finally, the Na@V/VOx @Al||NVP full cells were assembled
to investigate the practical application of the optimized foils in
SMBs. As expected, these full cells exhibit superior rate perfor-
mance compared to the Na@Al||NVP and Na@V@Al||NVP full
cells. As shown in Figure 7a, all cells exhibit high initial specific
capacities of ≈105mAh g−1 at 0.5 C. Upon increasing the dis-
charge rate to 20 C, the capacity of the Na@V/VOx @Al||NVP is
93 mAh g−1 , and it still can achieve 86 mAh g−1 even at 30 C.
In contrast, the discharge capacity of Na@V@Al||NVP cell drops
significantly to only 74 mAh g−1 at 30 C, and the Na@Al||NVP cell
experiences complete failure. From the charge-discharge curves
at different discharge rates (Figure 7b; Figure S16a,b, Support-
ing Information), it can be seen that the voltage polarization
of the Na@V/VOx @Al||NVP is much smaller than that of the
Na@Al||NVP and Na@V@Al||NVP. The excellent rate capabil-
ity and reduced voltage polarization of Na@V/VOx @Al||NVP in-
dicate that the heterostructure effectively enhances the trans-
port kinetics of Na+ . Figure S14 (Supporting Information) shows
the EIS spectra of different cells before cycling. Compared
with the Rct of Na@Al||NVP (≈131 Ω) and Na@V@Al||NVP
(≈63 Ω), Na@V/VOx @Al||NVP exhibits a smaller Rct (≈35 Ω),
which further confirms the improvement in Na+ transport ki-
netics achieved by the heterostructure. Additionally, the cycling
stability of Na@V/VOx @Al and other electrodes is compared
in Figure 7c and Figure S15 (Supporting Information). The
Na@V/VOx @Al shows the highest capacity of 102 mA h g−1
after 120 cycles at 1 C. When discharged at 10 C, the capacity

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Figure 7. a) Rate performance of different full cells. b) Charge-discharge voltage curve of the Na@V/VOx @Al||NVP full cell at various rates. c) Cycling
performance of different full cells at 10 C.
differences among the three electrodes became significant. The
Na@Al||NVP demonstrates an initial capacity of only 31 mAh
g−1 at 10 C, with a significant drop in capacity occurring af-
ter 960 cycles (Figure 7c). Similarly, the Na@V@Al||NVP ex-
periences a sharp decline in capacity after 850 cycles. How-
ever, the Na@V/VOx @Al||NVP maintains 97% capacity reten-
tion (Figure 7c) and an average CE of 98% after 1400 cycles at 10
C (Figure S16c, Supporting Information). Besides, their charge-
discharge curves at different cycling numbers (Figure S16d–f,
Supporting Information) also reveal the clear voltage plateau and
low polarization of the Na@V/VOx @Al||NVP, which indicate
that the V/VOx heterostructure enables the production of stable
and dendrite-free Na anode. Surprisingly, the Na@V/VOx @Al
electrode shows a long cycle life, which has obvious advantages
compared with previous reports (Table S3, Supporting Informa-
tion).
3. Conclusion
In summary, we successfully prepared the V/VOx @Al foil by
magnetron sputtering and calcination methods. Using advanced
characterization techniques such as XRD, XPS, and HRTEM,
we confirmed the successful construction of the heterostructure.
This unique heterostructure can be able to effectively enhance
Na+ transport kinetics, reduce the Na nucleation energy barrier,
and ultimately realize Na uniform deposition. To gain a deeper
understanding of its intrinsic mechanisms, we performed DFT
calculations. The calculation results reveal that the adsorption en-
ergy and charge transfer of Na+ on the V/VOx heterostructure are
strong, which is beneficial to reduce the overpotential of Na nu-
Adv. Funct. Mater. 2024, 2401914
16163028, 0, Downloaded from https://onlinelibrary.wiley.com/doi/10.1002/adfm.202401914 by Stanford University, Wiley Online Library on [01/04/2024]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
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cleation. And the FES results show that the V/VOx heterostruc-
ture can homogenize the current density distribution, provide
uniform nucleation sites for Na+ deposition, and realize uniform
and dense Na deposition. As a result, the V/VOx @Al electrode
can maintain a high average CE of 99.8% after 750 cycles and dis-
play a long cycle life (2750 h, 1 mA cm−2 ) in symmetrical cells.
More excitingly, the full cell assembled with Na@V/VOx @Al
electrode can be stably cycled for 1400 cycles and maintain 97%
capacity retention at 10 C. This work opens up possibilities for
the realization of SMBs with dendrite-free characteristic and long
cycle life.
Supporting Information
Supporting Information is available from the Wiley Online Library or from
the author.
Acknowledgements
This work was supported by the National Natural Science Founda-
tion of China (grant nos. 52222210, 51925207, U1910210, 52161145101,
51972067, 51902062, 52372239, 52102322, and 52002083), the Liaoning
Binhai Laboratory (Grant No. LBLF-2023-03), the National Synchrotron
Radiation Laboratory (grant no. KY2060000173), the Joint Fund of the Yulin
University and the Dalian National Laboratory for Clean Energy (grant no.
YLU-DNL Fund 2021002), and the Fundamental Research Funds for the
Central Universities (20720220010, WK2060000055, and WK2400000004).
Conflict of Interest
The authors declare no conflict of interest.
2401914 (8 of 9) © 2024 Wiley-VCH GmbH

www.advancedsciencenews.com
Data Availability Statement
The data that support the findings of this study are available from the cor-
responding author upon reasonable request.
Keywords
Al current collector, heterostructure, sodiophilicity, sodium dendrite,
sodium metal battery
Received: January 31, 2024
Revised: March 14, 2024
Published online:
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